Spark plasma sintering and thermoelectric evaluation of nanocrystalline magnesium silicide (Mg₂Si)

Recently magnesium silicide (Mg₂Si) has received great interest from thermoelectric (TE) society because of its non-toxicity, environmental friendliness, comparatively high abundance, and low production material cost as compared to other TE systems. It also exhibited promising transport properties, including high electrical conductivity and low thermal conductivity, which improved the overall TE performance (ZT). In this work, Mg₂Si powder was obtained through high energy ball milling under inert atmosphere, starting from commercial magnesium silicide pieces (99.99 %, Alfa Aesar). To maintain fine microstructure of the powder, spark plasma sintering (SPS) process has been used for consolidation. The Mg₂Si powder was filled in a graphite die to perform SPS and the influence of process parameters as temperature, heating rate, holding time and applied pressure on the microstructure, and densification of compacts were studied in detail. The aim of this study is to optimize SPS consolidation parameters for Mg₂Si powder to achieve high density of compacts while maintaining the nanostructure. X-Ray diffraction (XRD) was utilized to investigate the crystalline phase of compacted samples and scanning and transmission electron microscopy (SEM & TEM) coupled with Energy-Dispersive X-ray Analysis (EDX) was used to evaluate the detailed microstructural and chemical composition, respectively. All sintered samples showed compaction density up to 98 %. Temperature dependent TE characteristics of SPS compacted Mg₂Si as thermal conductivity, electrical resistivity, and Seebeck coefficient were measured over the temperature range of RT 600 °C for samples processed at 750 °C, reaching a final ZT of 0.14 at 600 °C.